Vertical Profiles Of Aerosol Extinction Research Articles

An iterative algorithm to simultaneously retrieve aerosol extinction and effective radius profiles using CALIOP

Abstract. The Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) on board the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite has been widely used in climate and environment studies to obtain the vertical profiles of atmospheric aerosols. To retrieve the vertical profile of aerosol extinction, the CALIOP algorithm assumes column-averaged lidar ratios based on a clustering of aerosol optical properties measured at surface stations. On one hand, these lidar ratio assumptions may not be appropriate or representative at certain locations. One the other hand, the two-wavelength design of CALIOP has the potential to constrain aerosol size information, which has not been considered in the operational algorithm. In this study, we present a modified inversion algorithm to simultaneously retrieve aerosol extinction and effective radius profiles using two-wavelength elastic lidars such as CALIOP. Specifically, a lookup table is built to relate the lidar ratio with the Ångström exponent calculated using aerosol extinction at the two wavelengths, and the lidar ratio is then determined iteratively without a priori assumptions. The retrieved two-wavelength extinction at each layer is then converted to the particle effective radius assuming a lognormal distribution. The algorithm is tested on synthetic data, Raman lidar measurements and then finally the real CALIOP backscatter measurements. Results show improvements over the CALIPSO operational algorithm by comparing with ground-based Raman lidar profiles.

Association between sea-land breeze and particulate matter in five coastal urban locations in India

Particulate matter less than 2.5 μm particle diameter (PM2.5) is the most significant environmental issue globally. PM2.5 is an integral component of air quality monitoring and management, human health, weather, climate, and epidemiological research. In this work, we investigate the seasonal variation in PM2.5 mass concentrations and the association between the sea-land breeze system and particulate matter in five coastal urban locations in India (Kolkata, Visakhapatnam, Chennai, Thiruvananthapuram, and Mumbai). The relative occurrence of high PM2.5 mass concentrations was the greatest during the winter season (December through February) while the relative occurrence of low PM2.5 mass concentrations was the greatest during the monsoon season (June through September). Amongst locations, Kolkata experiences the highest PM2.5 loading in winter while Thiruvananthapuram experiences the lowest PM2.5 loading in monsoon. Indo-Gangetic Plain (IGP) outflow onto the Bay of Bengal significantly impacts locations along the eastern coast of India with reduced impact from north (Kolkata) to south (Chennai). The sea-breeze component analysis revealed daily cycles of the sea-land breeze with varying magnitudes of the breeze between the different seasons. Overall, we found a negative association between the sea-land breeze magnitude and PM2.5 mass concentrations, implying that the weakened sea-land breeze may deteriorate air quality in coastal locations due to poor ventilation. The vertical profiles of aerosol extinction showed elevated aerosol layers within 1 km from the surface in almost all locations. The decreasing trend in the land-sea temperature contrast in coastal locations is expected to deteriorate air quality in coastal locations in the warming future. Nevertheless, critical analyses using ground-based remote sensing techniques are required for a better understanding the impact of sea-land breeze dynamics on air quality in coastal locations.

Martian Atmospheric Aerosols Composition and Distribution Retrievals During the First Martian Year of NOMAD/TGO Solar Occultation Measurements: 1. Methodology and Application to the MY 34 Global Dust Storm

AbstractSince the beginning of the Trace Gas Orbiter (TGO) science operations in April 2018, its instrument “Nadir and Occultation for MArs Discovery” (NOMAD) supplies detailed observations of the IR spectrums of the Martian atmosphere. We developed a procedure that allows us to evaluate the composition and distribution's parameters of the atmospheric Martian aerosols. We use a retrieval program (RCP) in conjunction with a radiative forward model (KOPRA) to evaluate the vertical profile of aerosol extinction from NOMAD measurements. We then apply a model/data fitting strategy of the aerosol extinction. In this first article, we describe the method used to evaluate the parameters representing the Martian aerosol composition and size distribution. MY 34 GDS showed a peak intensity from LS 190° to 210°. During this period, the aerosol content rises multiple scale height, reaching altitudes up to 100 km. The lowermost altitude of aerosol's detection during NOMAD observation rises up to 30 km. Dust aerosols reff were observed to be close to 1 μm and its νeff lower than 0.2. Water ice aerosols reff were observed to be submicron with a νeff lower than 0.2. The vertical aerosol structure can be divided in two parts. The lower layers are represented by higher reff than the upper layers. The change between the lower and upper layers is very steep, taking only few kilometers. The decaying phase of the GDS, LS 210°–260°, shows a decrease in altitude of the aerosol content but no meaningful difference in the observed aerosol's size distribution parameters.

Three-Dimensional Distribution of Biomass Burning Aerosols from Australian Wildfires Observed by TROPOMI Satellite Observations

We present a novel passive satellite remote sensing approach for observing the three-dimensional distribution of aerosols emitted from wildfires. This method, called AEROS5P, retrieves vertical profiles of aerosol extinction from cloud-free measurements of the TROPOMI satellite sensor onboard the Sentinel 5 Precursor mission. It uses a Tikhonov–Phillips regularization, which iteratively fits near-infrared and visible selected reflectances to simultaneously adjust the vertical distribution and abundance of aerosols. The information on the altitude of the aerosol layers is provided by TROPOMI measurements of the reflectance spectra at the oxygen A-band near 760 nm. In the present paper, we use this new approach for observing the daily evolution of the three-dimensional distribution of biomass burning aerosols emitted by Australian wildfires on 20–24 December 2019. Aerosol optical depths (AOD) derived by vertical integration of the aerosol extinction profiles retrieved by AEROS5P are compared with MODIS, VIIRS and AERONET coincident observations. They show a good agreement in the horizontal distribution of biomass burning aerosols, with a correlation coefficient of 0.87 and a mean absolute error of 0.2 with respect to VIIRS. Moderately lower correlations (0.63) were found between AODs from AEROS5P and MODIS, while the range of values for this comparison was less than half of that with respect to VIIRS. A fair agreement was found between coincident transects of vertical profiles of biomass burning aerosols derived from AEROS5P and from the CALIOP spaceborne lidar. The mean altitudes of these aerosols derived from these two measurements showed a good agreement, with a small mean bias (185 m) and a correlation coefficient of 0.83. Moreover, AEROS5P observations reveal the height of injection of the biomass burning aerosols in 3D. The highest injection heights during the period of analysis were coincident with the largest fire radiative power derived from MODIS. Consistency was also found with respect to the vertical stability of the atmosphere. The AEROS5P approach provides retrievals for cloud-free scenes over several regions, although currently limited to situations with a dominating presence of smoke particles. Future developments will also aim at observing other aerosol species.

Hourly Mapping of the Layer Height of Thick Smoke Plumes Over the Western U.S. in 2020 Severe Fire Season

A series of huge smoke plume events from the largest wildfire season recorded in California’s modern history has occurred in 2020. Here, a research algorithm was modified to retrieve the aerosol optical centroid height (AOCH) and aerosol optical depth (AOD) from Earth Polychromatic Imaging Camera (EPIC) measurements. The research focus is to gain insights of the algorithm’s feasibility in heavy smoke conditions to study the diurnal variation of AOCH; this is only made possible via EPIC due to its unique position at Lagrange-1 point and its equipment of O2 B-band at which the vegetated surface reflectance is low. Vicarious calibration is applied to the EPIC 443, 680 and 688 nm channels based on the Tropospheric Monitoring Instrument (TROPOMI) observation. This new calibration leads to a better agreement of AOCH values between EPIC retrievals and the counterparts derived from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) aerosol extinction vertical profile. The hourly variation of AOCH up to 0.45 km on September 7 is shown to have important implications for estimating hourly change of surface PM2.5, although more quantitative studies are needed in the future.

Investigation of the Influence of Water Vapor on Heavy Pollution and Its Relationship With AOD Using MAX‐DOAS on the Coast of the Yellow Sea

AbstractMulti‐AXis Differential Optical Absorption Spectroscopy (MAX‐DOAS) observations were carried out from March 1, 2019 to February 29, 2020 in Qingdao, China, on the coast of the Yellow Sea (120.67°E, 36.35°N). Atmospheric parameters retrieved from the MAX‐DOAS instrument included vertical profiles of aerosol extinction, gaseous aerosol precursors (NO2, SO2), and H2O. First, the seasonal relationship between aerosol optical depth (AOD) and the H2O vertical column density (VCD) was analyzed. The correlation coefficients (r) between AOD and H2O VCD were largest in the winter, followed by spring, autumn, and summer. In addition, the correlation during heavily polluted weather was much higher than that during clean weather or slightly polluted weather. Then, an analysis of the wind speed and direction, and trace gas VCDs during the months with frequent pollution (December 2019 and January 2020) found that heavy pollution episodes easily occurred in Qingdao due to a combination of high H2O concentrations and low wind speeds. Out of four pollution events (P1, P2, P3, P4), both the H2O concentration and pollution were highest during the first event (P1). The H2O VCD, AOD, sulfate AOD, and total column HNO3 simultaneously increased during P1, while the NO2 and SO2 VCDs decreased. These trends are consistent with liquid phase reactions. Finally, the 1,000 m backward trajectory for the wind and the gas profiles during P1 revealed that the pollutants increased in Qingdao due to the influence of a polluted air mass from the western inland regions.

Aerosol vertical distribution and interactions with land/sea breezes over the eastern coast of the Red Sea from lidar data and high-resolution WRF-Chem simulations

Abstract. With advances in modeling approaches and the application of satellite and ground-based data in dust-related research, our understanding of the dust cycle has significantly improved in recent decades. However, two aspects of the dust cycle, namely the vertical profiles and diurnal cycles, are not yet adequately understood, mainly due to the sparsity of direct observations. Measurements of backscattering caused by atmospheric aerosols have been ongoing since 2014 at the King Abdullah University of Science and Technology (KAUST) campus using a micro-pulse lidar (MPL) with a high temporal resolution. KAUST is located on the eastern coast of the Red Sea and currently hosts the only operating lidar system in the Arabian Peninsula. We use the data from the MPL together with other collocated observations and high-resolution simulations (with 1.33 km grid spacing) from the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) to study the following three aspects of dust over the Red Sea coastal plains. Firstly, we compare the model-simulated surface winds, aerosol optical depth (AOD), and aerosol size distributions with observations and evaluate the model performance in representing a typical large-scale dust event over the study site. Secondly, we investigate the vertical profiles of aerosol extinction and concentration in terms of their seasonal and diurnal variability. Thirdly, we explore the interactions between dust aerosols and land/sea breezes, which are the most influential components of the local diurnal circulation in the region. The WRF-Chem model successfully reproduced the diurnal profile of surface wind speed, AOD, and dust size distributions over the study area compared to observations. The model also captured the onset, demise, and height of a large-scale dust event that occurred in 2015, as compared to the lidar data. The vertical profiles of aerosol extinction in different seasons were largely consistent between the MPL data and WRF-Chem simulations along with key observations and reanalyses used in this study. We found a substantial variation in the vertical profile of aerosols in different seasons and between daytime and nighttime, as revealed by the MPL data. The MPL data also identified a prominent dust layer at ∼5–7 km during the nighttime, which likely represents the long-range transported dust brought to the site by the easterly flow from remote inland deserts. The sea breeze circulation was much deeper (∼2 km) than the land breeze circulation (∼1 km), but both breeze systems prominently affected the distribution of dust aerosols over the study site. We observed that sea breezes push the dust aerosols upwards along the western slope of the Sarawat Mountains. These sea breezes eventually collide with the dust-laden northeasterly trade winds coming from nearby inland deserts, thus causing elevated dust maxima at a height of ∼1.5 km above sea level over the mountains. Moreover, the sea and land breezes intensify dust emissions from the coastal region during the daytime and nighttime, respectively. Our study, although focused on a particular region, has broader environmental implications as it highlights how aerosols and dust emissions from the coastal plains can affect the Red Sea climate and marine habitats.

Measuring the Vertical Profiles of Aerosol Extinction in the Lower Troposphere by MAX-DOAS at a Rural Site in the North China Plain

Ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements were performed during the summer (13 June–20 August) of 2014 at a rural site in North China Plain. The vertical profiles of aerosol extinction (AE) in the lower troposphere were retrieved to analyze the temporal variations of AE profiles, near-surface AE, and aerosol optical depth (AOD). The average AOD and near-surface AE over the period of study were 0.51 ± 0.26 and 0.33 ± 0.18 km−1 during the effective observation period, respectively. High AE events and elevated AE layers were identified based on the time series of hourly AE profiles, near-surface AEs and AODs. It is found that in addition to the planetary boundary layer height (PBLH) and relative humidity (RH), the variations in the wind field have large impacts on the near-surface AE, AOD, and AE profile. Among 16 wind sectors, higher AOD or AE occur mostly in the directions of the cities upstream. The diurnal variations of the AE profiles, AODs and near-surface AEs are significant and influenced mainly by the source emissions, PBLH, and RH. The AE profile shape from MAX-DOAS measurement is generally in agreement with that from light detection and ranging (lidar) observations, although the AE absolute levels are different. Overall, ground-based MAX-DOAS can serve as a supplement to measure the AE vertical profiles in the lower troposphere.

Determination of Lidar Ratio for Major Aerosol Types over Western North Pacific Based on Long-Term MPLNET Data

East Asia is the most complex region in the world for aerosol studies, as it encounters a lot of varieties of aerosols, and aerosol classification can be a challenge in this region. In the present study, we focused on the relationship between aerosol types and aerosol optical properties. We analyzed the long-term (2005–2012) data of vertical profiles of aerosol extinction coefficients, lidar ratio (Sp), and other aerosol optical properties obtained from a NASA Micro-Pulse Lidar Network and Aerosol Robotic Network site in northern Taiwan, which frequently receives Asian continental outflows. Based on aerosol extinction vertical profiles, the profiles were classified into two types: type 1 (single-layer structure) and type 2 (two-layer structure). Fall season (October–November) was the prevailing season for the Type 1, whereas type 2 mainly happened in spring (March–April). In type 1, air masses normally originated from three regional sectors, i.e., Asia continental (AC), Pacific Ocean (PO), and Southeast Asia (SA). The mean Sp values were 39 ± 17 sr, 30 ± 12 sr, and 38 ± 18 sr for the AC, PO, and SA sectors, respectively. The Sp results suggested that aerosols from the AC sector contained dust and anthropogenic particles, and aerosols from the PO sector were most likely sea salts. We further combined the EPA dust event database and backward trajectory analysis for type 2. Results showed that Sp was 41 ± 14 sr and 53 ± 21 sr for dust storm and biomass-burning events, respectively. The Sp for biomass-burning events in type 2 showed two peaks patterns. The first peak occurred within range of 30–50 sr corresponding to urban pollutant, and the second peak occurred within range of 60–80 sr in relation to biomass burning. Finally, our study summarized the Sp values for four major aerosol types over northern Taiwan, viz., urban (42 ± 18 sr), dust (34 ± 6 sr), biomass-burning (69 ± 12 sr), and oceanic (30 ± 12 sr). Our findings provide useful references for aerosol classification and air pollution identification over the western North Pacific.

Validation of MAX-DOAS retrievals of aerosol extinction, SO<sub>2</sub>, and NO<sub>2</sub> through comparison with lidar, sun photometer, active DOAS, and aircraft measurements in the Athabasca oil sands region

Abstract. Vertical profiles of aerosols, NO2, and SO2 were retrieved from Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements at a field site in northern Alberta, Canada, during August and September 2013. The site is approximately 16 km north of two mining operations that are major sources of industrial pollution in the Athabasca oil sands region. Pollution conditions during the study ranged from atmospheric background conditions to heavily polluted with elevated plumes, according to the meteorology. This study aimed to evaluate the performance of the aerosol and trace gas retrievals through comparison with data from a suite of other instruments. Comparisons of aerosol optical depths (AODs) from MAX-DOAS aerosol retrievals, lidar vertical profiles of aerosol extinction, and the AERONET sun photometer indicate good performance by the MAX-DOAS retrievals. These comparisons and modelling of the lidar S ratio highlight the need for accurate knowledge of the temporal variation in the S ratio when comparing MAX-DOAS and lidar data. Comparisons of MAX-DOAS NO2 and SO2 retrievals to Pandora spectral sun photometer vertical column densities (VCDs) and active DOAS mixing ratios indicate good performance of the retrievals, except when vertical profiles of pollutants within the boundary layer varied rapidly, temporally, and spatially. Near-surface retrievals tended to overestimate active DOAS mixing ratios. The MAX-DOAS observed elevated pollution plumes not observed by the active DOAS, highlighting one of the instrument's main advantages. Aircraft measurements of SO2 were used to validate retrieved vertical profiles of SO2. Advantages of the MAX-DOAS instrument include increasing sensitivity towards the surface and the ability to simultaneously retrieve vertical profiles of aerosols and trace gases without requiring additional parameters, such as the S ratio. This complex dataset provided a rare opportunity to evaluate the performance of the MAX-DOAS retrievals under varying atmospheric conditions.

Method to retrieve aerosol extinction profiles and aerosol scattering phase functions with a modified CCD laser atmospheric detection system.

Vertical distributions of ambient aerosols and their corresponding optical properties are crucial to the assessment of aerosol radiative effects. Traditionally, ambient aerosol phase function is assumed as a constant of input parameter in the retrieval of the vertical distribution of aerosol optical characteristics from remote sensing measurements (e.g. lidar or camera-laser based instruments). In this work, sensitivity studies revealed that using constant aerosol phase function assumptions in the algorithm would cause large uncertainties. Therefore, an improved retrieval method was established to simultaneously measure ambient aerosol scattering phase functions and aerosol scattering function profiles with a modified charge-coupled device-laser aerosol detection system (CLADS), which are then combined to yield vertical profiles of aerosol extinction coefficients. This method was applied and evaluated in a comprehensive field campaign in the North China Plain during January 2016. The algorithm showed robust performance and was able to capture temporal variations in ambient aerosol scattering phase functions and aerosol scattering function profiles. Aerosol extinction coefficients derived with simultaneously measured aerosol phase functions agreed well with in-situ measurements, indicating that uncertainties in the retrieval of aerosol extinction vertical profiles have been significantly reduced by using the proposed method with the modified CLADS. The advantage of this modified CLADS is that it can accomplish these aerosol measurements independent of other supplementary instruments. Benefiting from its low cost and high spatial resolution (∼1 m on average) in the boundary layer, this measurement system can play an important role in the research of aerosol vertical distributions and its impacts on environmental and climatic studies.

Evaluation of retrieved aerosol extinction profiles using as reference the aerosol optical depth differences between various heights

Aerosol extinction vertical profiles at Granada (Spain) are calculated with the GRASP (Generalized Retrieval of Aerosol and Surface Properties) code using as input Aerosol Optical Depth (AOD) and sky radiance measurements from AERONET (AEerosol RObotic NETwork) and ceilometer RCS (Range Corrected Signal) profiles, both corresponding to the Granada (Spain) station. This methodology is so called GRASPpac due to the combination of sun/sky photometer and ceilometer on GRASP. In order to evaluate the accuracy of these retrieved extinction profiles at Granada, two more nearby AERONET stations, located at different altitudes, are used. The AOD difference of the three choosen AERONET sun/sky photometers have been used to calculate the Integrated Aerosol Extinction (IAE) at different height layers. These three AERONET sun/sky photometers are used as a reference and compared against the integrated extinction at the same layers from the extinction profiles retrieved by GRASPpac. The differences between AERONET and GRASPpac retrieved IAE values indicate that GRASPpac aerosol extinction profiles are at least within the uncertainty of the sun/sky photometer measurements, but GRASPpac method overestimates the AERONET extinction at low altitudes and underestimates it at high levels. The most accurate and precise retrieved extinction correspond to the intermediate layer with a mean bias error (MBE ± standard deviation) of 0.00 ± 0.01 (0 ± 59%) for 1020 nm, and the worst integrated extinction results were obtained for the upper layers with a MBE of −0.01 ± 0.02 (28 ± 36%) for 1020 nm. In general these MBE values increases for shorter wavelengths. In order to obtain a complete characterization of this bias, the dependence of the obtained differences on the aerosol size and the solar zenith angle, among others, are analysed in detail. Finally, the behaviour of vertically-resolved aerosol extinction at Granada is evaluated using averages of the retrieved profiles from November of 2012 to December of 2017. The highest IAE values are found in Summer with mean values of 0.09 for the lower layers and 0.07 for the upper ones, both at 440 nm wavelength.

Vertical profile of aerosol extinction based on the measurement of O4 of multi-elevation angles with MAX-DOAS**Project supported by the National Natural Science Foundation of China (Grant Nos. 41875040, 41705012, and 1605013).

A method for aerosol extinction profile retrieval using ground-based multi-axis differential optical absorption spectroscopy (MAX-DOAS) is studied, which is based on a look-up table algorithm. The algorithm uses parametric method to represent aerosol extinction profiles and simulate different atmospheric aerosol states through atmospheric radiation transfer model. Based on the method, aerosol extinction profile was obtained during six cloud-free days. The O4 differential air mass factor (dAMF) measured by MAX-DOAS is compared with the corresponding model results under different atmospheric conditions (). The aerosol optical thickness, aerosol weight factor in boundary layer, and the height of the boundary layer are obtained after the process of minimization and look-up table method. The retrieved aerosol extinction in boundary layer is compared with PM2.5 data measured by ground point instrument. The diurnal variation trends of the two methods are in good agreement. The correlation coefficients of the two methods are 0.71 when the aerosol optical thickness is smaller than 0.5. The results show that the look-up table method can obtain the aerosol state of the troposphere and provide validation for other instrument data.

The Mainz profile algorithm (MAPA)

Abstract. The Mainz profile algorithm (MAPA) derives vertical profiles of aerosol extinction and trace gas concentrations from MAX-DOAS measurements of slant column densities under multiple elevation angles. This paper presents (a) a detailed description of the MAPA (v0.98), (b) results for the CINDI-2 campaign, and (c) sensitivity studies on the impact of a priori assumptions such as flag thresholds. Like previous profile retrieval schemes developed at MPIC, MAPA is based on a profile parameterization combining box profiles, which also might be lifted, and exponential profiles. But in contrast to previous inversion schemes based on least-square fits, MAPA follows a Monte Carlo approach for deriving those profile parameters yielding best match to the MAX-DOAS observations. This is much faster and directly provides physically meaningful distributions of profile parameters. In addition, MAPA includes an elaborated flagging scheme for the identification of questionable or dubious results. The AODs derived with MAPA for the CINDI-2 campaign show good agreement with AERONET if a scaling factor of 0.8 is applied for O4, and the respective NO2 and HCHO surface mixing ratios match those derived from coincident long-path DOAS measurements. MAPA results are robust with respect to modifications of the a priori MAPA settings within plausible limits.

Optimization of the lidar optical design for measurement of the aerosol extinction vertical profile

A lidar for aerosol monitoring with conventional optical design can provide good quality signals from several hundred meters up to tens of kilometres above the ground, but the aerosol load is mainly contained (up to 80%) in the planetary boundary layer that can have a height of only hundreds of meters above the ground level. Therefore, the measurement of the complete aerosol extinction profile is generally a very difficult challenge. In this paper, we proposed an optical design of lidar systems able of producing signals starting from a few tens of meters above the ground. The overlap profiles obtained from an optimized lidar was compared with ray tracing simulations and further conventional lidar apparatuses.

Aerosol optical properties derived from POLDER-3/PARASOL (2005–2013) over the western Mediterranean Sea – Part 1: Quality assessment with AERONET and in situ airborne observations

Abstract. The western Mediterranean atmosphere is impacted by a variety of aerosol sources, producing a complex and variable mixture of natural and anthropogenic particles, with different chemical and physical properties. Satellite sensors provide a useful global coverage of aerosol parameters but through indirect measurements that require careful validation. Here we present the results of a long-term regional scale analysis of the full dataset (March 2005 and October 2013) of POLDER-3/PARASOL ocean operational retrievals of the total, fine, and coarse aerosol optical depth (AOD, AODF, and AODC), Ångström exponent (AE), and the spherical or non-spherical partition of coarse-mode AOD (AODCS and AODCNS), respectively. The evaluation is performed using data from 17 coastal and insular ground-based AERONET sites on one side, and airborne vertical profiles of aerosol extinction and number size distribution obtained by the SAFIRE ATR-42 aircraft operated in the area during summer 2012 and 2013 on the other side. This study provides the first regional evaluation of uncertainties of the POLDER-3 products, and highlights their quality. The POLDER-3 Ångström exponent, representing AOD spectral dependence in link with the aerosol particle size distribution, is biased towards small values. This bias, however, does not prevent using AE for classifying the regional aerosol laden air masses. AODF corresponds to particles smaller than 0.6–0.8 µm in diameter and appears suitable to monitor the aerosol submicron fraction from space. We also provide an original validation of POLDER-3 AODC and its spherical or non-spherical partition, which shows agreement within 25 % with AERONET shape retrievals when the aerosol coarse fraction dominates.

Comparing multiple model-derived aerosol optical properties to spatially collocated ground-based and satellite measurements

Abstract. Anthropogenic aerosols are a key factor governing Earth's climate and play a central role in human-caused climate change. However, because of aerosols' complex physical, optical, and dynamical properties, aerosols are one of the most uncertain aspects of climate modeling. Fortunately, aerosol measurement networks over the past few decades have led to the establishment of long-term observations for numerous locations worldwide. Further, the availability of datasets from several different measurement techniques (such as ground-based and satellite instruments) can help scientists increasingly improve modeling efforts. This study explores the value of evaluating several model-simulated aerosol properties with data from spatially collocated instruments. We compare aerosol optical depth (AOD; total, scattering, and absorption), single-scattering albedo (SSA), Ångström exponent (α), and extinction vertical profiles in two prominent global climate models (Geophysical Fluid Dynamics Laboratory, GFDL, CM2.1 and CM3) to seasonal observations from collocated instruments (AErosol RObotic NETwork, AERONET, and Cloud–Aerosol Lidar with Orthogonal Polarization, CALIOP) at seven polluted and biomass burning regions worldwide. We find that a multi-parameter evaluation provides key insights on model biases, data from collocated instruments can reveal underlying aerosol-governing physics, column properties wash out important vertical distinctions, and improved models does not mean all aspects are improved. We conclude that it is important to make use of all available data (parameters and instruments) when evaluating aerosol properties derived by models.

Intercomparison of aerosol extinction profiles retrieved from MAX-DOAS measurements

Abstract. A first direct intercomparison of aerosol vertical profiles from Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) observations, performed during the Cabauw Intercomparison Campaign of Nitrogen Dioxide measuring Instruments (CINDI) in summer 2009, is presented. Five out of 14 participants of the CINDI campaign reported aerosol extinction profiles and aerosol optical thickness (AOT) as deduced from observations of differential slant column densities of the oxygen collision complex (O4) at different elevation angles. Aerosol extinction vertical profiles and AOT are compared to backscatter profiles from a ceilometer instrument and to sun photometer measurements, respectively. Furthermore, the near-surface aerosol extinction coefficient is compared to in situ measurements of a humidity-controlled nephelometer and dry aerosol absorption measurements. The participants of this intercomparison exercise use different approaches for the retrieval of aerosol information, including the retrieval of the full vertical profile using optimal estimation and a parametrised approach with a prescribed profile shape. Despite these large conceptual differences, and also differences in the wavelength of the observed O4 absorption band, good agreement in terms of the vertical structure of aerosols within the boundary layer is achieved between the aerosol extinction profiles retrieved by the different groups and the backscatter profiles observed by the ceilometer instrument. AOTs from MAX-DOAS and sun photometer show a good correlation (R>0.8), but all participants systematically underestimate the AOT. Substantial differences between the near-surface aerosol extinction from MAX-DOAS and from the humidified nephelometer remain largely unresolved.

Trans-Pacific transport and evolution of aerosols: evaluation of quasi-global WRF-Chem simulation with multiple observations

Abstract. A fully coupled meteorology-chemistry model (WRF-Chem, the Weather Research and Forecasting model coupled with chemistry) has been configured to conduct quasi-global simulation for 5 years (2010–2014) and evaluated with multiple observation data sets for the first time. The evaluation focuses on the simulation over the trans-Pacific transport region using various reanalysis and observational data sets for meteorological fields and aerosol properties. The simulation generally captures the overall spatial and seasonal variability of satellite retrieved aerosol optical depth (AOD) and absorbing AOD (AAOD) over the Pacific that is determined by the outflow of pollutants and dust and the emissions of marine aerosols. The assessment of simulated extinction Ångström exponent (EAE) indicates that the model generally reproduces the variability of aerosol size distributions as seen by satellites. In addition, the vertical profile of aerosol extinction and its seasonality over the Pacific are also well simulated. The difference between the simulation and satellite retrievals can be mainly attributed to model biases in estimating marine aerosol emissions as well as the satellite sampling and retrieval uncertainties. Compared with the surface measurements over the western USA, the model reasonably simulates the observed magnitude and seasonality of dust, sulfate, and nitrate surface concentrations, but significantly underestimates the peak surface concentrations of carbonaceous aerosol likely due to model biases in the spatial and temporal variability of biomass burning emissions and secondary organic aerosol (SOA) production. A sensitivity simulation shows that the trans-Pacific transported dust, sulfate, and nitrate can make significant contribution to surface concentrations over the rural areas of the western USA, while the peaks of carbonaceous aerosol surface concentrations are dominated by the North American emissions. Both the retrievals and simulation show small interannual variability of aerosol characteristics for 2010–2014 averaged over three Pacific sub-regions. The evaluation in this study demonstrates that the WRF-Chem quasi-global simulation can be used for investigating trans-Pacific transport of aerosols and providing reasonable inflow chemical boundaries for the western USA, allowing one to further understand the impact of transported pollutants on the regional air quality and climate with high-resolution nested regional modeling.

Influence of the vertical absorption profile of mixed Asian dust plumes on aerosol direct radiative forcing over East Asia

We estimate the aerosol direct radiative forcing (ADRF) and heating rate profiles of mixed East Asian dust plumes in the solar wavelength region ranging from 0.25 to 4.0 μm using the Santa Barbara Discrete Ordinate Atmospheric Radiative Transfer (SBDART) code. Vertical profiles of aerosol extinction coefficients and single-scattering albedos (SSA) were derived from measurements with a multi-wavelength Raman lidar system. The data are used as input parameters for our radiative transfer calculations. We considered four cases of radiative forcing in SBDART: 1. dust, 2. pollution, 3. mixed dust plume and the use of vertical profiles of SSA, and 4. mixed dust plumes and the use of column-averaged values of SSA. In our sensitivity study we examined the influence of SSA and aerosol layer height on our results. The ADRF at the surface and in the atmosphere shows a small dependence on the specific shape of the aerosol extinction vertical profile and its light-absorption property for all four cases. In contrast, at the top of the atmosphere (TOA), the ADRF is largely affected by the vertical distribution of the aerosols extinction. This effect increases if the light-absorption capacity (decrease of SSA) of the aerosols increases. We find different radiative effects in situations in which two layers of aerosols had different light-absorption properties. The largest difference was observed at the TOA for an absorbing aerosol layer at high altitude in which we considered in one case the vertical profile of SSA and in another case the column-averaged SSA only. The ADRF at the TOA increases when the light-absorbing aerosol layer is located above 3 km altitude. The differences between height-resolved SSA, which can be obtained from lidar data, and total layer-mean SSA indicates that the use of a layer-mean SSA can be rather misleading as it can induce a large error in the calculation of the ADRF at the TOA, which in turn may cause errors in the vertical profiles of heating rates.